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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 901 records · Page 50
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Evidence for Interfacial Halogen Bonding

Abstract A homologous series of donor–π–acceptor dyes was synthesized, differing only in the identity of the halogen substituents about the triphenylamine (TPA; donor) portion of each molecule. Each Dye‐X (X=F, Cl, Br, and I) was immobilized on a TiO 2 surface to investigate how the halogen substituents affect the reaction between the light‐induced charge‐separated state, TiO 2 (e − )/ Dye‐X + , with iodide in solution. Transient absorption spectroscopy showed progressively faster reactivity towards nucleophilic iodide with more polarizable halogen substituents: Dye‐F < Dye‐Cl < Dye‐Br < Dye‐I . Given that all other structural and electronic properties for the series are held at parity, with the exception of an increasingly larger electropositive σ‐hole on the heavier halogens, the differences in dye regeneration kinetics for Dye‐Cl , Dye‐Br , and Dye‐I are ascribed to the extent of halogen bonding with the nucleophilic solution species.

Swords, Wesley B.↗
DOE OSTI2016

Evidence for Interfacial Halogen Bonding

Abstract A homologous series of donor–π–acceptor dyes was synthesized, differing only in the identity of the halogen substituents about the triphenylamine (TPA; donor) portion of each molecule. Each Dye‐X (X=F, Cl, Br, and I) was immobilized on a TiO 2 surface to investigate how the halogen substituents affect the reaction between the light‐induced charge‐separated state, TiO 2 (e − )/ Dye‐X + , with iodide in solution. Transient absorption spectroscopy showed progressively faster reactivity towards nucleophilic iodide with more polarizable halogen substituents: Dye‐F < Dye‐Cl < Dye‐Br < Dye‐I . Given that all other structural and electronic properties for the series are held at parity, with the exception of an increasingly larger electropositive σ‐hole on the heavier halogens, the differences in dye regeneration kinetics for Dye‐Cl , Dye‐Br , and Dye‐I are ascribed to the extent of halogen bonding with the nucleophilic solution species.

Swords, Wesley B.↗
DOE OSTI2023

Enhanced Photo-Cross-Linking of Thymines in DNA Holliday Junction-Templated Squaraine Dimers

Programmable self-assembly of dyes using DNA templates to promote exciton delocalization in dye aggregates is gaining considerable interest. New methods to improve the rigidity of the DNA scaffold and thus the stability of the molecular dye aggregates to encourage exciton delocalization are desired. In these dye–DNA constructs, one potential way to increase the stability of the aggregates is to create an additional covalent bond via photo-cross-linking reactions between thymines in the DNA scaffold. Specifically, we report an approach to increase the yield of photo-cross-linking reaction between thymines in the core of a DNA Holliday junction while limiting the damage from UV irradiation to DNA. We investigated the effect of the distance between thymines on the photo-cross-linking reaction yields by using linkers with different lengths to tether the dyes to the DNA templates. By comprehensively evaluating the photo-cross-linking reaction yields of dye–DNA aggregates using linkers with different lengths, we conclude that interstrand thymines tend to photo-cross-link more efficiently with short linkers. A higher cross-linking yield was achieved due to the shorter intermolecular distance between thymines influenced by strong dye–dye interactions. Furthermore, our method establishes the possibility of improving the stability of DNA-scaffolded dye aggregates, thereby expanding their use in exciton-based applications such as light harvesting, nanoscale computing, quantum computing, and optoelectronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Exciton Delocalization in Indolenine Squaraine Aggregates Templated by DNA Holliday Junction Scaffolds

Exciton delocalization plays a prominent role in the photophysics of molecular aggregates, ultimately governing their particular function or application. DNA is a compelling scaffold in which to template molecular aggregates and promote exciton delocalization. As individual dye molecules are the basis of exciton delocalization in molecular aggregates, their judicious selection is important. Motivated by their excellent photostability and spectral properties, here we examine the ability of squaraine dyes to undergo exciton delocalization when aggregated via a DNA Holliday junction (HJ) template. A commercially available indolenine squaraine dye was chosen for the study given its strong structural resemblance to Cy5, a commercially available cyanine dye previously shown to undergo exciton delocalization in DNA HJs. Three types of DNA-dye aggregate configurations—transverse dimer, adjacent dimer, and tetramer—were investigated. Signatures of exciton delocalization were observed in all squaraine-DNA aggregates. Specifically, strong blue shift and Davydov splitting were observed in steady-state absorption spectroscopy and exciton-induced features were evident in circular dichroism spectroscopy. Strongly suppressed fluorescence emission provided additional, indirect evidence for exciton delocalization in the DNA-templated squaraine dye aggregates. To quantitatively evaluate and directly compare the excitonic Coulombic coupling responsible for exciton delocalization, the strength of excitonic hopping interactions between the dyes were obtained by simultaneous fitting the experimental steady-state absorption and CD spectra via a Holstein-like Hamiltonian in which, following the theoretical approach of Kühn, Renger, and May, the dominant vibrational mode is explicitly considered. The excitonic hopping strength within indolenine squaraines was found to be comparable to that of the analogous Cy5 DNA-templated aggregate. The squaraine aggregates adopted primarily an H-type (dyes oriented parallel to each other) spatial arrangement. Extracted geometric details of dye mutual orientation in the aggregates enabled close comparison of aggregate configurations and the elucidation of the influence of dye angular relationship on excitonic hopping interactions in squaraine aggregates. Furthermore, these results encourage the application of squaraine-based aggregates in next generation systems driven by molecular excitons.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Bright emissive core-shell spherical microparticles for shock compression spectroscopy

Experiments were performed to study the response to shock compression of rhodamine 6G (R6G) dye encapsulated in 1.25 μm diameter silica microspheres. When R6G was encapsulated in microspheres, the emission intensity under steady-state irradiation (the brightness) was 3.4 times greater than the same dye in solution (the free dye). At least part of the brightness improvement was caused by an enhanced radiative rate. When the microspheres were embedded in poly-methylmethacrylate subjected to planar shocks in the 3–8.4 GPa range by laser-driven flyer plates, the dye emission redshifted and lost intensity. The dye emission redshift represents an instantaneous response to changes in the local density. In free dye samples, the shock-induced intensity loss had considerably slower rise times and fall times than the redshift. When dye was encapsulated in microspheres, the time dependence of the intensity loss matched the redshift almost exactly over a range of shock pressures and durations. The faster response to shock of dye in silica microspheres was explained by dye photophysics. The microsphere environment decreased the singlet state lifetime, which decreased the rise time, and it also decreased the triplet state lifetime, which decreased the fall time. Since it is much easier and more convenient to make measurements of intensity rather than spectral shift, these microspheres represent a substantial improvement in optical sensors to monitor shock compression of microstructured materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Adsorption of Methylene Blue, Brilliant Green and Rhodamine B from Aqueous Solution Using Collagen-g-p(AA-co-NVP)/Fe{sub 3}O{sub 4}@SiO{sub 2} Nanocomposite Hydrogel

In this study, the collagen-g-poly(acrylic acid-co-N-vinylpyrrolidone)/Fe{sub 3}O{sub 4}@SiO{sub 2} (collagen-g-p(AA-co-NVP)/Fe{sub 3}O{sub 4}@SiO{sub 2}) as magnetic nanocomposite hydrogel was synthesized by graft copolymerization of acrylic acid (AA) and N-vinylpyrrolidone (NVP) onto collagen in the presence of the Fe{sub 3}O{sub 4}@SiO{sub 2} using ammonium persulfate as a free radical initiator and bis[2-(methacryloyloxy)ethyl] phosphate as a crosslinker under ultrasound-assisted condition. The blank collagen-g-p(AA-co-NVP) hydrogel and its composite with the Fe{sub 3}O{sub 4}@SiO{sub 2} nanoparticles were characterized by means of FTIR, SEM-EDS, XRD, VSM and TGA methods. The effects of different parameters such as pH, dose of adsorbent and time on swelling behavior were examined. The swelling ratio of the collagen-g-p(AA-co-NVP) hydrogel increased in the presence of the Fe{sub 3}O{sub 4}@SiO{sub 2} nanoparticles. Adsorption behavior of magnetic nanocomposite hydrogel was investigated for the adsorption of dyes and it was found to remove about 93% for methylene blue, 96% for brilliant green and 89% for rhodamine B in 50 mg/L of dyes solutions at pH 7. Kinetic study revealed the applicability of pseudo-first-order and pseudo-second-order models for the adsorption of mentioned dyes. The adsorption isotherm was studied in 25, 35, 45 and 55 °C using Langmuir, Freundlich, Temkin and Sips models and the adsorption data were well described by Langmuir isotherm model. Negative values of ΔG{sup º} for all three dyes suggested the feasibility of dyes removal and support for spontaneous adsorption of mentioned dyes on magnetic nanocomposite hydrogel. Desorption of dyes from the dye loaded nanocomposite hydrogel was simply done in ethanol. The results indicate that the prepared magnetic nanocomposite hydrogel is an efficient adsorbent with high adsorption capacity for the aforementioned dyes.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2019

Effect of extending conjugation via thiophene-based oligomers on the excited state electron transfer rates to ZnO nanocrystals

Oligothiophene dyes with two to five thiophene units were anchored to oleate-capped, quantum-confined zinc oxide nanocrystals (ZnO NCs) through a cyanoacrylate functional group. While the fluorescence of the bithiophene derivative was too weak for meaningful quenching studies, the fluorescence of the dyes with three, four and five thiophene rings was quenched upon binding to the NCs. Ultrafast pump–probe spectroscopy was used to observe the singlet excited states of the free dyes dissolved in dichloromethane as well as attached to a ZnO NC dispersed in the same solvent. When the dyes were bound to ZnO NCs, ultrafast spectroscopic measurements revealed rapid disappearance of the singlet excited state and appearance of a new transient absorption at higher energy that was assigned to the oxidized dye based on the similar absorption observed upon oxidation of the dye using nitrosonium ion. The appearance lifetimes of the oxidized dyes were assigned to the excited state electron transfer and were 36 ± 2, 22.3 ± 3.9, 26.5 ± 1.5 and 19.4 ± 0.8 ps for bi-, ter-, quarter- and quinquethiophene dyes respectively. Two factors contributed to the similarity in the electron transfer lifetime. First the excited state energies of the dyes were similar, and second, the free energy for electron transfer reaction was sufficiently large to move the event into the energy-independent regime.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Plastic scintillator with effective pulse shape discrimination for neutron and gamma detection

In one embodiment, a scintillator material includes a polymer matrix; and a primary dye in the polymer matrix, the primary dye being a fluorescent dye, the primary dye being present in an amount of 5 wt % or more; wherein the scintillator material exhibits an optical response signature for neutrons that is different than an optical response signature for gamma rays. In another embodiment, a scintillator material includes a polymer matrix comprising at least one of: polyvinyl xylene (PVX); polyvinyl diphenyl; and polyvinyl tetrahydronaphthalene; and a primary dye in the polymer matrix, the primary dye being a fluorescent dye, the primary dye being present in an amount greater than 10 wt %. A total loading of dye in the scintillator material is sufficient to cause the scintillator material to exhibit a pulse-shape discrimination (PSD) figure of merit (FOM) of about at least 2.0.

Zaitseva, Natalia P.↗
DOE OSTI2018

Improving Quantum Yield of Upconverting Nanoparticles in Aqueous Media via Emission Sensitization

We demonstrate a facile method to improve upconversion quantum yields in Yb,Er-based nanoparticles via emission dye-sensitization. Using the commercially available dye ATTO 542, chosen for its high radiative rate and significant spectral overlap with the green emission of Er 3+ , we decorate the surfaces of sub-25 nm hexagonal-phase Na(Y/Gd/Lu) 0.8 F 4 :Yb 0.18 Er 0.02 upconverting nanoparticles with varying dye concentrations. Upconversion photoluminescence and absorption spectroscopy provide experimental confirmation of energy transfer to and emission from the dye molecules. Upconversion quantum yield is observed to increase with dye sensitization, with the highest enhancement measured for the smallest particles investigated (10.9 nm in diameter); specifically, these dye-decorated particles are more than 2× brighter than are unmodified, organic-soluble nanoparticles and more than 10× brighter than are water-soluble nanoparticles. We also observe 3× lifetime reductions with dye adsorption, confirming the quantum yield enhancement to result from the high radiative rate of the dye. As a result, the approach detailed in this work is widely implementable, renders the nanoparticles water-soluble, and most significantly improves sub-15 nm nanoparticles, making our method especially attractive for biological imaging applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Controlling Interfacial Charge Separation Energetics and Kinetics

The overall goal is to probe electron transfer kinetics of the Marcus inverted region at interfaces. This project specifically uses a dye‐semiconductor interface with a reversible electron transfer reagent in solution where the semiconductor conduction band and electron transfer reagent ideally have a potential energy difference firmly within the Marcus inverted region. The goals of this project are: (Goal 1) Identify dye design elements that give dyes with low energy ground‐state oxidation potentials while retaining desirable electron transfer kinetics at the semiconductor interface. (Goal 2) Identify dye designs with excited‐state oxidation potentials set to fixed energies through molecular design while the dye ground‐state oxidation potentials are varied to allow for the evaluation of varied electron transfer reagents/redox shuttles (RS) with different free energies for electron transfer. (Goal 3) Within the context of the functionality identified in goals 1 and 2, goal 3 seeks to design dyes with features maximizing charge carrier lifetimes by minimizing recombination losses at metal oxide interfaces with high voltage systems. (Goal 4) Probe electron transfer kinetics in a high voltage‐dye sensitized solar cell with both the oxidized dye and RS firmly within the Marcus inverted region with regard to the TiO2 CB. (Goal 5) Identify tailored sensitizer/redox shuttle pairs with desirable electron transfer kinetics in defined spectral regions capable of “banding off” incident solar irradiation to give high voltage multijunction systems capable of exceeding the Shockley‐Queisser limit and powering catalytic processes.

14 SOLAR ENERGY↗
DOE OSTI2016

Plastic scintillator with effective pulse shape discrimination for neutron and gamma detection

In one embodiment, a scintillator material includes a polymer matrix; and a primary dye in the polymer matrix, the primary dye being a fluorescent dye, the primary dye being present in an amount of 5 wt % or more; wherein the scintillator material exhibits an optical response signature for neutrons that is different than an optical response signature for gamma rays. In another embodiment, a scintillator material includes a polymer matrix; and a primary dye in the polymer matrix, the primary dye being a fluorescent dye, the primary dye being present in an amount greater than 10 wt %.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Investigation of the decolorization efficiency of two pin-to-plate corona discharge plasma system for industrial wastewater treatment

In this article, a dual pin-to-plate high-voltage corona discharge system is introduced to study experimentally the gap distance, the contact time, the effect of pin and plate materials, the thickness of ground plate and the conductivity on the amount of Acid Blue 25 dye color removal efficiency from polluted water. A study for the optimum air gap distance between dual pin and surface of Acid Blue 25 dye solution is carried out using 3D-EM simulator to find maximum electric field intensity at the tip of both pins. The outcomes display that the best gap for corona discharge is approximately 5 mm for 15-kV source. This separation is constant during the study of other factors. In addition, an investigation of the essential reactive species responsible for oxidation of the dye organic compounds (O{sub 3} in air discharge, O{sub 3} in water, and H{sub 2}O{sub 2}) during the experimental time is conducted. Three various materials such as: stainless steel, copper and aluminum are used for pins and plate. The maximum color removal efficiencies of Acid Blue 25 dyes are 99.03, 82.04, and 90.78% after treatment time 15 min for stainless steel, copper, and aluminum, respectively. Measurement results for the impact of thickness of an aluminum ground plate on color removal competence show color removal efficiencies of 86.3, 90.78, and 98.06% after treatment time 15 min for thicknesses of 2, 0.5, and 0.1 mm, respectively. The increasing of the solution conductivity leads to the reduction of decolorization efficiency. A kinetic model is used to define the performance of corona discharge system. The models of pseudo-zero-order, pseudo-first-order, and pseudo-second-order reaction kinetics are utilized to investigate the decolorization of Acid Blue 25 dye. The rate of degradation of Acid Blue 25 dye follows the pseudo-first-order kinetics in the dye concentration.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Effect of Solvent and Substrate on the Surface Binding Mode of Carboxylate-Functionalized Aromatic Molecules

Here, the efficiency of dye-sensitized solar cells (DSSCs) is strongly influenced by dye molecule orientation and interactions with the substrate. Understanding the factors controlling the surface orientation of sensitizing organic molecules will aid in the improvement of both traditional DSSCs and other devices that integrate molecular linkers at interfaces. Here, we describe a general approach to understand relative dye–substrate orientation and provide analytical expressions predicting orientation. We consider the effects of substrate, solvent, and protonation state on dye molecule orientation. In the absence of solvent, our model predicts that most carboxylic acid-functionalized molecules prefer to lie flat (parallel) on the surface, due to van der Waals interactions, as opposed to a tilted orientation with respect to the surface that is favored by covalent bonding of the carboxylic acid group to the substrate. When solvation effects are considered, however, the molecules are predicted to orient perpendicular to the surface. We extend this approach to help understand and guide the orientation of metal–organic framework (MOF) thin-film growth on various metal–oxide substrates. A two-part analytical model is developed on the basis of the results of DFT calculations and ab initio MD simulations that predicts the binding energy of a molecule by chemical and dispersion forces on rutile and anatase TiO 2 surfaces, and quantifies the dye solvation energy for two solvents. The model is in good agreement with the DFT calculations and enables rapid prediction of dye molecule and MOF linker binding preference on the basis of the size of the adsorbing molecule, identity of the surface, and the solvent environment. We establish the threshold molecular size, governing dye molecule orientation, for each condition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Electronic and chemical structure of an organic light emitter embedded in an inorganic wide-bandgap semiconductor: Photoelectron spectroscopy of layered and composite structures of Ir(BPA) and ZnSe

Luminescent organic phases embedded in conductive inorganic matrices are proposed for hybrid organic-inorganic light-emitting diodes. In this configuration, the organic dye acts as the radiative recombination site for charge carriers injected into the inorganic matrix. Our investigation is aimed at finding a material combination where the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) of the organic dye are situated in between the valence and conduction bands of the inorganic matrix in order to promote electron and hole transfer from the matrix to the dye. Bilayer and composite thin films of zinc selenide (ZnSe) and a red iridium complex (Ir(BPA)) organic light emitter were prepared in situ via UHV thermal evaporation technique. The electronic and atomic structures were studied applying X-ray and ultraviolet photoelectron spectroscopies. The measured energy band alignments for the ZnSe/Ir(BPA) bilayer and ZnSe+Ir(BPA) composite reveal that the HOMO and LUMO of the organic dye are positioned in the ZnSe bandgap. For the initial steps of ZnSe deposition on a dye film to form Ir(BPA)/ZnSe bilayers, zinc atoms intercalate into the dye film leaving behind an excess of selenium at the interface that partly reacts with dye molecules. Photoelectron spectroscopy of the composites shows the same species suggesting a similar mechanism. This mechanism leads to composite films with increased content of amorphous phases in the inorganic matrix, thereby affecting its conductivity, as well as to the presence of nonradiative recombination sites provided by the intercalated Zn atoms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS2000

Optical Sensors Based on Single on Arm Thin Film Waveguide Interferometer

Single-arm dual-mode optical waveguide interferometer utilizes interference between two modes of different order. Sensing effect results from the change in propagation conditions of the modes caused by the environment. The waveguide is made as an open asymmetric structure containing a dye-doped polymer film onto a quartz substrate. It is more sensitive to the change of environment than its conventional polarimetric analog using orthogonal modes (TE and TM) of the same order. The sensor still preserves the option of operating in polarimetric regime using a variety of mode combinations such as TE(sub 0)/TM(sub 0) (conventional) TE(sub 0)/TM(sub 1), TE(sub 1)/TM(sub 0), or TE(sub 1)/TM(sub 1) but can also work in nonpolarimetric regime using combinations TE(sub 0)/TE(sub 1) or TM(sub 0)/TM(sub 1). Utilization of different mode combinations simultaneously makes the device more versatile. Application of the sensor to gas sensing is based on doping polymer film with an organic indicator dye targeting a particular gaseous reagent. Change of the optical absorption spectrum of the dye caused by the gaseous pollutant results in change of the reactive index of the dye-doped polymer film that can be detected by the sensor. As indicator dyes we utilize Bromocresol Purple doped into polymer poly(methyl) methacrylate that is sensitive to small concentrations of ammonia. The indicator dye demonstrated an irreversible increase in optical absorption near the peak at 350 nm being exposed to 5% ammonia in pure nitrogen at 600 Torr. The dye also showed reversible growth of the absorption peak near 600 nm after exposure to a vapor of standard medical ammonia spirit (65% alcohol). We have built a breadboard prototype of the sensor with He-Ne laser as a light source and with a single mode fiber input and a multimode fiber output. The prototype showed a sensitivity to temperature change of the order of 2 C per 2pi phase shift. The sensitivity of the sensor to the presence of dTy ammonia is not less than 300 ppm per 2pi phase shift. The proposed sensor can be used as a robust stand-alone instrument for continuous environment pollution monitoring.

Sarkisov, S. S.↗
DOE OSTI2018

Design-to-Device Approach Affords Panchromatic Co-sensitized Solar Cells

Data–driven materials discovery has become increasingly important in identifying materials that exhibit specific, desirable properties from a vast chemical search space. Synergic prediction and experimental validation are needed to accelerate scientific advances related to critical societal applications. A design–to–device study that uses high–throughput screens with algorithmic encodings of structure–property relationships is reported to identify new materials with panchromatic optical absorption, whose photovoltaic device applications are then experimentally verified. The data–mining methods source 9431 dye candidates, which are auto–generated from the literature using a custom text–mining tool. These candidates are sifted via a data–mining workflow that is tailored to identify optimal combinations of organic dyes that have complementary optical absorption properties such that they can harvest all available sunlight when acting as co–sensitizers for dye–sensitized solar cells (DSSCs). Six promising dye combinations are shortlisted for device testing, whereupon one dye combination yields co–sensitized DSSCs with power conversion efficiencies comparable to those of the high–performance, organometallic dye, N719. Here, these results demonstrate how data–driven molecular engineering can accelerate materials discovery for panchromatic photovoltaic or other applications.

14 SOLAR ENERGY↗
DOE OSTI2018

Spectral Properties and Possibilities of meso-Substituted BODIPY Usage in Sol–Gel Process and Materials

Hybrid materials based on organically modified silica with immobilized boron-dipyrrins (BODIPY) dyes were obtained. Spectral characteristics of the dyes were measured during the matrix formation and in obtained materials. It was stated, that immobilization does not affect the character of the absorption and fluorescence spectra of the dye, but due to the effect of fluorescent molecular rotor observed for meso-substituted BODIPY, the fluorescent quantum yields were found to increase during the matrix sealing. Quantum yield increase is linear for all of the investigated matrices except phenyl-substituted one, where the π-π interactions of the dye molecule with matrix could be observed. This effect could be used for fine control of the matrix formation process and leads to increase of the dye emission in the final material for further practical applications. All obtained hybrid materials were found to be stable upon UV light irradiation, hence immobilization enhance the stability of the dye in comparison with the BODIPY in organic solvents.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Photophysics of “Floppy” Dyads as Potential Biomembrane Probes

In the study a dyad (C6 probe), constructed of two dyes with highly different hydrophobicities, was investigated by steady-state and time-resolved spectroscopic techniques in chloroform, methanol, and in phospholipid vesicles, respectively. The dyad was built on two dyes: the lipophilic benzo[a]pyrene (BaP) and the hydrophilic sulforhodamine B (SRB). The dyes were linked via a short, but flexible alkyl chain (six C-atoms). Based on their spectroscopic properties, BaP and SRB showed a very efficient non-radiative resonance energy transfer in solution. Incorporation into a lipid bilayer limited the relative flexibility (degree of freedom) between donor and acceptor and was used for the investigation of fundamental photophysical aspects (especially of FRET) as well as to elucidate the potential of the dyad to probe the interface of vesicles (or cells). The location of the two dyes in vesicles and their respective accessibility for interactions with dye-specific antibodies was investigated. Based on the alteration of the anisotropy, on the rotational correlation time as well as on the diffusion coefficient the incorporation of the C6 probe into the vesicles was evaluated. Especially the limitation in the relative movements of the two dyes was considered and used to differentiate between potential parameters, that influence the energy transfer in the dyad. Transient absorption spectroscopy (TAS) and pulsed-interleave single molecule fluorescence experiments were performed to better understand the intramolecular interactions in the dyad. Finally, in a showcase for a biosensing application of the dyads, the binding of an SRB-specific antibody was investigated when the dyad was incorporated in vesicles. .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗